The effect of a slight A- and B-site cation nonstoichiometry on the structure, densification, and
microwave dielectric properties of Ba(Mg1/ 3Ta2/3)O3 (BMT) was investigated. Magnesium and barium
nonstoichiometric compositions based on Ba(Mg0.33
-
x
Ta0.67)O3 [x = −0.015, −0.010, −0.005, 0.0, 0.005,
0.010, 0.015, 0.020, 0.025, and 0.030] and Ba1
-
x
(Mg0.33Ta0.67)O3 [x = −0.015, −0.010, −0.005, 0.0,
0.0025, 0.005, 0.0075, 0.010, 0.015, 0.020, 0.025, and 0.030] were prepared using the conventional solid-state ceramic route. The lattice distortion and cation ordering were determined using X-ray diffraction
technique. The phase composition and surface morphology were studied by EDX and scanning electron
microscopy techniques, respectively. The sintered samples were characterized in the microwave frequency
range using the resonance technique. It is found that a slight barium or magnesium deficiency can improve
density, microwave dielectric properties, and cation ordering, while the addition of excess ions deteriorated
them. The improvement in microwave dielectric properties was more pronounced in barium nonstoichiometric samples. Microwave dielectric properties of Ba0.9925(Mg0.33Ta0.67)O3 [εr = 24.7, τf = 1.2 ppm/°C, Quxf = 152 580 GHz] and Ba(Mg0.3183Ta0.67)O3 [εr = 25.1, τf = 3.3 ppm/°C and Quxf = 120 500
GHz] were found to be better than stoichiometric BMT [εr = 24.2, τf = 8 ppm/°C and Quxf = 100 500
GHz]. Raman spectroscopy was employed to study the effects of nonstoichiometry and related lattice
distortions in BMT ceramics on their vibrational modes. Raman results clearly showed the 1:2 ordered
structures of these materials with all active modes assigned. The spectra showed variations in the normal
modes as a function of the composition. Also secondary phases contributed to the changes in the Raman
spectra observed in compounds with x ≥ 0.02.